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DOE OSTI2025

Simulation of Physics-Based 0-10Hz Strong Motion Using High Performance Computing Supporting Refinements to Regional Ground Motion Models for the Central Eastern US

In collaboration with the U.S. Nuclear Regulatory Commission (NRC) the LLNL has developed a computationally efficient simulation platform designed to perform physics-based ground motion simulations for crustal earthquakes in the Stable Continental Regions of Central and Eastern US (CEUS), using high-performance computing. The main objective of the earthquake simulations was to use synthetic ground motion to provide constrains to refinements of existing ergodic Ground Motion Models (GMMs), for large magnitude earthquakes and near-fault distances, for which these models are less reliable. Physics-based broadband (0-10Hz) ground motion simulations were used to estimate the near-fault ground motion amplitudes and within event and between-event variabilities associated with fault rupture characteristics. In our simulations we used a 3D regional velocity model that was based on Saikia’s 1D velocity model (1994). In simulations performed during the first stage of this project the Saikia’s velocity model demonstrated better performance in modelling high frequency regional wave propagation for the CEUS region recorded during the Mw5.0 November 7, 2016, Cushing Oklahoma (Taylor et al., 2017), and Mw5.8 September 3, 2016, Pawnee Oklahoma earthquakes. The proposed regional 3D model includes random perturbations to the 1D background model using the stochastic scheme of Pitarka and Mellors (2021). In addition, validation analysis of the rupture generator and regional wave propagation models, using comparisons with different GMMs for Mw6.5 and Mw7.0 scenario earthquakes in the CEUS region resulted in a very good match between the simulated and empirical ground motion models. For the purposes of seismic hazard assessment at the existing and planned nuclear power plants, NRC is interested in studies aimed at improving the current ground motion models (GMM) for both Stable Continental Regions (SCR) in the Central and Eastern US and Active Crustal Regions (ACR) in the Western US. Due to lack of recorded data, these improvements require synthetic data for short fault distances and large magnitude earthquakes for which the existing recorded data is not enough to uniquely constrain the GMMs. The need for simulations and strong motion data is especially critical for the CEUS region where we do not have recorded data from potentially large damaging earthquakes with moment magnitudes 6.0 and higher. In this the project, we focused on 10Hz simulations of Mw7.0 scenario earthquakes with strike slip and thrust faulting mechanisms. We used more than 50 Mw7.0 earthquake rupture scenarios to investigate the ground motion uncertainty due to unknown earthquake rupture parameters, in particular, the slip distribution, rupture velocity, and faulting mechanism, and their implication on ground motion amplification due to forward rupture directivity effects.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2025

Towards the Stable Chelation of Radioantimony(V) for Targeted Auger Theranostics

Abstract Antimony‐119 ( 119 Sb) is one of the most attractive Auger‐electron emitters identified to date, but it remains practically unexplored for targeted radiotherapy because no chelators have been identified to stably bind this metalloid in vivo. In a departure from current studies focused on chelator development for Sb(III), we explore the chelation chemistry of Sb(V) using the tris‐catecholate ligand TREN‐CAM. Through a combination of radiolabeling, spectroscopic, solid‐state, and computational studies, the radiochemistry and structural chemistry of TREN‐CAM with 1XX/nat Sb(V) were established. The resulting [ 1XX Sb]Sb–TREN‐CAM complex remained intact for several days in human serum, signifying high stability under biological conditions. Finally, the first in vivo single photon emission computed tomography and positron emission tomography imaging studies were carried out using 117 Sb, the diagnostic analogue of 119 Sb. These studies revealed marked differences in the uptake and distribution of activity in mice administered unchelated [ 117 Sb]Sb(OH) 6 – versus [ 117 Sb]Sb–TREN‐CAM, suggesting that 117 Sb is largely retained by TREN‐CAM over the time course of the study. Collectively, these findings demonstrate the most physiologically stable complex of no‐carrier‐added 1XX Sb yet reported, offering new promise for the clinical implementation of radioantimony in nuclear medicine. Our results also establish the feasibility of 117 Sb as an elementally matched partner to 119 Sb for theranostic applications.

Olson, Aeli P. [Department of Medical Physics Univ↗

DOE OSTI2021

Predicting and Synthesizing Interface Stabilized 2D Layers

The compound (Pb 2 MnSe 3 ) 0.6 VSe 2 was predicted to be kinetically stable based on density functional theory (DFT) calculations on an island of Pb 2 MnSe 3 between layers of VSe 2 . This approach provides a high degree of freedom by not forcing interlayer lattice match, making it ideal to investigate the likelihood of formation of new incommensurate layer misfit structures. The free space around the island is critical, as it allows atoms to diffuse and hence exploring the local energy landscape around the initial configuration. (Pb 2 MnSe 3 ) 0.6 VSe 2 was synthesized via a near diffusionless reaction from precursors where a repeating sequence of elemental layers matches the local composition and layer sequence of the predicted compound. The VSe 2 layer consists of a Se–V–Se trilayer with octahedral coordination of the V atoms. The Pb 2 MnSe 3 layer consists of three rock-salt-like planes, with a MnSe layer between the planes of PbSe. The center MnSe plane stabilizes the puckering of the outer PbSe layers. Electrical properties indicate that (Pb 2 Mn 1 Se 3 ) 0.6 VSe 2 undergoes a charge density wave transition at ~100 K and orders ferromagnetically at 35 K. Overall, the combination of theory and experiment enables a faster convergence to new heterostructures than either approach in isolation.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Neutron occupancies and single-particle energies across the stable tin isotopes

The occupancies and vacancies of the valence neutron orbitals across the stable tin isotopic chain from 112 ≤ A ≤ 124 have been determined. These were inferred from the cross sections of neutron adding and -removing reactions. In each case, the reactions were chosen to have good angular momentum matching for transfer to the low- and high-` orbitals present in this valence space. Here, these new data are compared to older systematic studies. The effective single-neutron energies are determined by combining information from energy centroids determined from the adding and removing reactions. Two of the five orbitals are nearly degenerate, below N = 64, and approximately two MeV more bound than the other three, which are also degenerate.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2026

Stable and tunable MeV $$\gamma$$-ray generation via dual-laser inverse Thomson scattering from a laser-plasma accelerator

Abstract Inverse Thomson scattering from laser-plasma accelerators offers a pathway to compact, tunable MeV $$\gamma$$ -ray sources for reduced-dose radiography and enhanced performance in nuclear resonance fluorescence (NRF)-based isotope identification. However, photon yield and spectral quality are often limited by constraints on interaction geometry and scatter-laser tunability. Here we demonstrate a MeV $$\gamma$$ -ray source based on a dual-laser inverse Thomson scattering configuration driven by a 100-TW laser-plasma accelerator. Electron beams tunable from 122 to 204 MeV with $$<5$$ mrad divergence and $$<1$$ mrad pointing stability generate $$\gamma$$ rays with peak energies from 276 keV to 1.2 MeV and yields up to $$2\times 10^{7}$$ photons per shot. By independently controlling the interaction position and the scatter-pulse duration, we experimentally match the scatter pulse to the walk-off-limited interaction length. Extending the scatter pulse to 200 fs increases photon production by approximately $$15\%$$ while maintaining operation in the linear Thomson regime, thereby preserving narrow spectral bandwidth and controlled radiation divergence. Radiographic characterization demonstrates MeV-level penetration and $$\approx 0.1$$ mm spatial resolution, while stable operation is sustained over multi-hour timescales across multiple days. These results show that interaction-length optimization provides a scalable strategy for improving photon yield, spectral control, and operational stability in compact laser-plasma-accelerator-driven $$\gamma$$ -ray sources.

Tsai, Hai-En↗

DOE OSTI2023

Decoupling Accurate Electrochemical Behaviors for High-Capacity Electrodes via Reviving Three-Electrode Vehicles

Developing high-capacity electrodes requires the evaluation of electrochemical behaviors with an increasing current density. Currently, the current density for evaluation of high-capacity electrodes has reached a new stage where the polarization at the lithium counter electrode has become a technical barrier for the accurate evaluation of battery electrodes, resulting in severe performance and mechanism mischaracterizations. Here, the accurate electrochemical behavior for high-capacity electrodes via a single-channel three-electrode vehicle is decoupled, by which the impact of lithium counter electrode is minimized. The testing high-capacity graphite electrode is capable of delivering an excellent rate capability with 81.7% capacity retention at 0.3 C, as well as stable cycling performance retaining 97.5% practical reversible capacity after 225 cycles, much higher than the graphite electrode tested with traditional half-cell testing vehicle but in close agreement with the results obtained from a well-matched full cell, reflecting accurate electrochemical performance evaluations of high-capacity electrodes. Moreover, detailed electrochemical mechanisms of impedance and diffusion properties for working electrodes are also successfully decoupled individually. Here, this work uncovers the mismatch between traditional evaluation configuration and increasing testing current density and provides a guideline for accurate electrochemical evaluation for ever-increasing high-capacity electrodes, which is of great significance for high-energy lithium or other alkali-metal ion batteries.

25 ENERGY STORAGE↗

DOE OSTI2025

Towards the Stable Chelation of Radioantimony(V) for Targeted Auger Theranostics

Antimony-119 ( 119 Sb) is one of the most attractive Auger-electron emitters identified to date, but it remains practically unexplored for targeted radiotherapy because no chelators have been identified to stably bind this metalloid in vivo. In a departure from current studies focused on chelator development for Sb(III), we explore the chelation chemistry of Sb(V) using the tris-catecholate ligand TREN-CAM. Through a combination of radiolabeling, spectroscopic, solid-state, and computational studies, the radiochemistry and structural chemistry of TREN-CAM with 1XX/nat Sb(V) were established. The resulting [ 1XX Sb]Sb–TREN-CAM complex remained intact for several days in human serum, signifying high stability under biological conditions. Finally, the first in vivo single photon emission computed tomography and positron emission tomography imaging studies were carried out using 117 Sb, the diagnostic analogue of 119 Sb. These studies revealed marked differences in the uptake and distribution of activity in mice administered unchelated [ 117 Sb]Sb(OH) 6 – versus [ 117 Sb]Sb–TREN-CAM, suggesting that 117 Sb is largely retained by TREN-CAM over the time course of the study. Collectively, these findings demonstrate the most physiologically stable complex of no-carrier-added 1XX Sb yet reported, offering new promise for the clinical implementation of radioantimony in nuclear medicine. In conclusion, our results also establish the feasibility of 117 Sb as an elementally matched partner to 119 Sb for theranostic applications.

62 RADIOLOGY AND NUCLEAR MEDICINE↗

DOE OSTI2024

Lignin Deoxygenation for the Production of Sustainable Aviation Fuel Blendstocks

Lignin is an abundant source of renewable aromatics that has long been targeted for valorization. Traditionally, the inherent heterogeneity and reactivity of lignin has relegated it to direct combustion, but its higher energy density compared with polysaccharides makes it an ideal candidate for biofuel production. This Review critically assesses lignin's potential as a substrate for sustainable aviation fuel blendstocks. Lignin can generate the necessary cyclic compounds for a fully renewable, sustainable aviation fuel when integrated with current paraffinic blends and can meet the current demand 2.5 times over. Using an energy-centric analysis, we show that lignin conversion technologies have the near-term potential to match the enthalpic yields of existing commercial sustainable aviation fuel production processes. Key factors influencing the viability of technologies for converting lignin to sustainable aviation fuel include lignin structure, delignification extent, depolymerization performance, and the development of stable and tunable deoxygenation catalysts.

09 BIOMASS FUELS↗

DOE OSTI2021

Redox-stable symmetrical solid oxide fuel cells with exceptionally high performance enabled by electrode/electrolyte diffuse interface

Here, in this study, we report a high performance and redox-stable symmetrical solid oxide fuel cell (SOFC) based on (Ba 0.5 Sr 0.5 ) (Mo 0.1 Fe 0.9 )O 3-δ (BSMF) electrode and La 0.8 Sr 0.2 Ga 0.8 Mg 0.2 O 3-δ (LSGM) electrolyte. BSMF is able to operate both as anode and cathode. Excellent electrocatalytic activity has been achieved on BSMF towards hydrogen oxidation and oxygen reduction. Due to its closely matched lattice parameter to LSGM electrolyte, a unique diffuse interface is formed between BSMF and LSGM. Compared to a clean interface, e.g. BSMF/gadolinium doped ceria interface, this diffuse interface promotes the performance of BSMF electrode 1–1.8 times in 600–800 °C. Polarization resistance of the BSMF/LSGM specimen is as low as 0.047 and 0.007 Ωcm 2 in humidified H 2 and in air at 800 °C, respectively. On the BSMF/LSGM/BSMF symmetrical cell, a maximum power density of 2.28 W/cm 2 is achieved at 800 °C, the highest among with redox-stable ceramic electrodes to the best of our knowledge. Redox stability of this cell is confirmed. The role of anode and cathode is reversed back and forth in different operation modes. No apparent degradation is observed through 4 cycles within a 110 h operation period. These findings demonstrate that (Ba 0.5 Sr 0.5 ) (M o0.1 Fe 0.9 )O 3-δ coupled with LSGM electrolyte is an excellent choice to build a high performance, redox-stable SOFC.

25 ENERGY STORAGE↗

DOE OSTI2022

Resolving atomistic structure and oxygen evolution activity in nickel antimonates

The oxygen evolution reaction (OER) requires electrodes that are not only catalytically active, but also stable under harsh electrochemical environments to enable efficient, durable technologies. Our recent report of a stable amorphous Ni 0.5 Sb 0.5 O z OER photoanode established Ni–Sb–O as an important system for computational understanding of both the structural and catalytic behavior of these complex oxides. In the present work we show that Ni x Sb 1-x O z with x > 0.33 crystallizes into a previously unknown phase. Guided by experimental X-ray diffraction, here, we use density functional theory calculations to perform a prototype phase search to identify a broad family of stable and metastable mixed rutile and hexagonal-like phases for x = 0.33, 0.50, and 0.66 compositions. For the identified phases, we predict favorable oxygen vacancy formation energies for Ni-rich compositions under the reducing synthesis conditions which match measured Ni K-edge X-ray absorption spectra. The calculated overpotential for the most active site decreases with increasing Ni content, from 0.91 V (x = 0.33) to 0.49 V (x = 0.66), which captures the experimentally observed trend. We find the active site changes from the Ni–O–Sb bridge to a Ni–O–Ni bridge at increasing Ni concentrations, rather than the commonly studied singly under-coordinated sites. Finally, detailed Pourbaix analysis of the identified phases show excellent electrochemical stability, consistent with experimentally measured low metal ion concentrations in the electrolyte of photoelectrochemical cells. Collectively, our consideration of an ensemble of structures enables identification of the most catalytically prolific structural motifs, aiding the understanding of crystalline and amorphous catalysts and elucidating the co-optimization of activity and durability in nickel antimonates.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

A path to scaling helium-3 spin-exchange optical pumping

Polarized 3 He has contributed to breakthroughs in particle physics, neutron scattering, and lung imaging, mostly by optical pumping of liter quantities in valved cells or in sealed cells pumped in situ. Only metastability exchange optical pumping currently meets the demand for delivering large quantities of highly polarized 3 He to external volumes. Our development program is under way to achieve medium to large-scale spin-exchange optical pumping of 3 He. Thin-walled aluminosilicate cells placed in contact with thermal reservoirs inside a pressure vessel were optically pumped with kilowatt-scale lasers spectrally narrowed to match pressure-broadened absorption linewidths. We report here the key elements of this program and significant milestones: multi-liter volume valved cells that provide long longitudinal lifetimes that reached polarization as high as 85% inside a thermally stable and pressurized environment.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2020

A High-efficacy CRISPRi System for Gene Function Discovery in Zymomonas mobilis

Zymomonas mobilis is a promising biofuel producer due to its high alcohol tolerance and streamlined metabolism that efficiently converts sugar to ethanol. Z. mobilis genes are poorly characterized relative to those of model bacteria, hampering our ability to rationally engineer the genome with pathways capable of converting sugars from plant hydrolysates into valuable biofuels and bioproducts. Many of the unique properties that make Z. mobilis an attractive biofuel producer are controlled by essential genes; however, these genes cannot be manipulated using traditional genetic approaches (e.g., deletion or transposon insertion) because they are required for viability. CRISPR interference (CRISPRi) is a programmable gene knockdown system that can precisely control the timing and extent of gene repression, thus enabling targeting of essential genes. Here, we establish a stable, high-efficacy CRISPRi system in Z. mobilis that is capable of perturbing all genes—including essential genes. We show that Z. mobilis CRISPRi causes either strong knockdowns (>100-fold) using single guide RNA (sgRNA) spacers that perfectly match target genes or partial knockdowns using spacers with mismatches. We demonstrate the efficacy of Z. mobilis CRISPRi by targeting essential genes that are universally conserved in bacteria, are key to the efficient metabolism of Z. mobilis, or underlie alcohol tolerance. Our Z. mobilis CRISPRi system will enable comprehensive gene function discovery, opening a path to rational design of biofuel production strains with improved yields.

lignocellulosic hydrolysate↗

DOE OSTI2021

First principles study of the stability and thermal conductivity of novel Li-Be hybrid ceramics

Hybrid Li-Be ceramics, combining both tritium (T) breeder (Li) and neutron multiplier (Be) for use as part of the fuel cycle of future nuclear fusion reactors are proposed. The development of such hybrid materials may reduce thermal gradients through better matching of thermal properties, mitigating the detrimental effects that may accompany traditional breeder systems while maintaining acceptable neutron multiplication and T breeding. Here, first-principles methods are used to investigate stability and thermal transport properties of a set of compounds containing both Li and Be. It is demonstrated that BeLi 2 O 4 Ge and BeLi 2 O 4 Si are mechanically stable and have formation energies comparable with leading candidates for solid state breeder materials, Li 2 TiO 3 , Li 2 ZrO 3 . It is also demonstrated that similar to the leading candidates, these compounds are insulators with thermal transport defined by phonons. The calculated thermal conductivity of BeLi 2 O 4 Ge is slightly higher compared to Li 2 TiO 3 or Li 2 ZrO 3 while in the BeLi 2 O 4 Si it is almost three times higher compared to the rest of compounds due to a higher phonon group velocities and increased phonon lifetimes. These results indicate that hybrid Li-Be ceramics offer a potential route towards better matching of thermal properties with minimal functional property degradation, thereby offering better overall fuel cycle performance.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Novel Amorphous Carbons for the Adsorption of Phosphate: Part I. Elucidation of Chemical Structure of N-Metal-Doped Chars

Due to phosphate’s necessity in agriculture and its danger to the environment, the development of adsorbents for its removal has been the subject of intensive research activity. Although the introduction of nitrogen functionality to chars and modification of biochar with metals have proven to change the character of the char structure, making it more active toward nutrients, there is no study regarding the doping of biochar with metals and nitrogen simultaneously for the adsorption of phosphates. This paper is the first of two in which we report the production, characterization, and evaluation of N-metal-doped biochars from cellulose for phosphate removal from liquid effluents. In this part, we describe the production and characterization of N-Ca-, N-Fe-, and N-Mg-doped biochars. The elemental composition and surface area of each of the materials produced is reported. Elemental and surface characterization of the chars are reported with the largest N content appearing at a temperature of 800 °C (12.5 wt %) and a maximum surface area for biochar produced at 900 °C (1314 m2/g). All of the adsorbents were visualized by scanning electron microscope (SEM), confirming that although there are some crystals on the surface of the biochar produced, most of the N, Mg, and Ca are part of the polyaromatic ring structure. Transmission electron microscope (TEM) images clearly show the formation of nanoclusters with the metals in the case of N-Fe and N-Ca biochars. The N-Mg biochars show a uniform distribution of the Mg through the carbon surface. X-ray photoelectron spectroscopy (XPS) studies of the biochars produced with metals and varying nitrogen levels clearly show Mg and Ca peaks shifting their position in the presence of N, suggesting the formation of stable structures between metals and N in the carbon polyaromatic ring system. To elucidate the nature of these structures, we conducted DFT-based calculations on different configurations of the nitrogenated structures. The calculated binding energy shifts were found to closely match the XPS experimental binding energy, confirming the likelihood of these structures in biochar. Finally, based on our experimental and modeling results, we hypothesize that an important fraction of the Mg and Ca is introduced to these biochars at the edges. Another fraction of Mg and Ca is in the form of phthalocyanine-like internal structures. More experimental studies are needed to confirm the formation of these very interesting structures and their potential use as adsorbents or catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Electrodes with silicon oxide active materials for lithium ion cells achieving high capacity, high energy density and long cycle life performance

Improved negative electrodes can comprise a silicon based active material blended with graphite to provide more stable cycling at high energy densities. In some embodiments, the negative electrodes comprise a blend of polyimide binder mixed with a more elastic polymer binder with a nanoscale carbon conductive additive. The silicon-based blended graphite negative electrodes can be matched with positive electrodes comprising nickel rich lithium nickel manganese cobalt oxides to form high energy density cells with good cycling properties.

Venkatachalam, Subramanian↗

DOE OSTI2023

Electrodes with silicon oxide active materials for lithium ion cells achieving high capacity, high energy density and long cycle life performance

Venkatachalam, Subramanian↗

DOE OSTI2021

Plug-and-play polymer microfluidic chips for hydrated, room temperature, fixed-target serial crystallography

The practice of serial X-ray crystallography (SX) depends on efficient, continuous delivery of hydrated protein crystals while minimizing background scattering. Of the two major types of sample delivery devices, fixed-target devices offer several advantages over widely adopted jet injectors, including: lower sample consumption, clog-free delivery, and the ability to control on-chip crystal density to improve hit rates. In this study we present our development of versatile, inexpensive, and robust polymer microfluidic chips for routine and reliable room temperature serial measurements at both synchrotrons and X-ray free electron lasers (XFELs). Our design includes highly X-ray-transparent enclosing thin film layers tuned to minimize scatter background, adaptable sample flow layers tuned to match crystal size, and a large sample area compatible with both raster scanning and rotation based serial data collection. The optically transparent chips can be used both for in situ protein crystallization (to eliminate crystal handling) or crystal slurry loading, with prepared samples stable for weeks in a humidified environment and for several hours in ambient conditions. Serial oscillation crystallography, using a multi-crystal rotational data collection approach, at a microfocus synchrotron beamline (SSRL, beamline 12-1) was used to benchmark the performance of the chips. Furthermore, high-resolution structures (1.3–2.7 Å) were collected from five different proteins – hen egg white lysozyme, thaumatin, bovine liver catalase, concanavalin-A (type VI), and SARS-CoV-2 nonstructural protein NSP5. Overall, our modular fabrication approach enables precise control over the cross-section of materials in the X-ray beam path and facilitates chip adaption to different sample and beamline requirements for user-friendly, straightforward diffraction measurements at room temperature.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2024

MARVEL Corrosion Test Interim Report

This study explores eutectic gallium-indium-tin (e-GaInSn) as a potential coolant for the intermediate heat exchanger for the MARVEL microreactor. E-GaInSn has an exceptionally low melting point of 10.8 °C and a high boiling point exceeding 1300 °C [4]. This wide temperature range provides designers with a significant margin to coolant boiling, even under severe accident conditions. Moreover, e-GaInSn is highly stable in both air and water demonstrating a high coefficient of thermal conductivity compared to conventional coolants like water or polymer-based solutions, along with a large heat capacity and low vapor pressure [5, 6]. While its heat transfer characteristics may not match those of some other liquid metals such as sodium, they are still quite favorable [6]. More importantly, gallium does not present issues related to chemical activity in a nuclear reactor environment. These unique and advantageous properties make e-GaInSn an attractive option for reactor applications. However, it is essential to thoroughly evaluate the compatibility of E-GaInSn with structural materials, particularly steels, for which it has a relatively high affinity. Presently, the compatibility data for these liquid metals or alloys with candidate structural materials remains limited, underscoring the need for further research to ascertain their suitability as liquid breeders or coolants [7

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗